The electrical performance of solution-processed, small-molecule organic semiconductors is largely restricted by their severe charge carrier mobility variations. In this work, we demonstrate an effective method to reduce such variations of the semiconductor mobilities and improve the performance consistency of organic thin film transistors (OTFTs) by adding poly(α-methylstyrene) (PαMS) as a polymer additive. By using 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS pentacene) as an example, we found that while pristine TIPS pentacene film exhibited random crystal orientation and large film gaps, the addition of PαMS polymer promoted the growth of semiconductor crystals, which formed uniformly aligned needles with significantly improved orientation and coverage within the channel regions. An ultra-low misorientation angle of 2.2° ± 1° was obtained from TIPS pentacene/PαMS blend film, which is a 20-fold reduction as compared to pristine TIPS pentacene. Bottom-gate, top-contact OTFTs with TIPS pentacene crystals aligned perpendicularly from source to drain contact electrodes demonstrated a hole mobility of up to 0.26 cm2/V s, as well a 6-fold enhancement of average mobility as compared to the pristine TIPS pentacene based counterparts. Notably, the addition of PαMS led to a performance consistency factor of 3.35, as defined by the ratio of the average mobility to standard deviation, implying a great reduction of charge carrier mobility variations. The improvement of electrical performance of OTFTs can be attributed to the combined outcome of crystal rigid alignment, extended long-range order, and almost full coverage of charge transport channel.